Zhang Fu, Lu Yanfu, Schulman Daniel S, Zhang Tianyi, Fujisawa Kazunori, Lin Zhong, Lei Yu, Elias Ana Laura, Das Saptarshi, Sinnott Susan B, Terrones Mauricio
Department of Materials Science and Engineering, The Pennsylvania State University, University Park, PA 16802, USA.
Center for Two-Dimensional and Layered Materials, The Pennsylvania State University, University Park, PA 16802, USA.
Sci Adv. 2019 May 24;5(5):eaav5003. doi: 10.1126/sciadv.aav5003. eCollection 2019 May.
Chemical doping constitutes an effective route to alter the electronic, chemical, and optical properties of two-dimensional transition metal dichalcogenides (2D-TMDs). We used a plasma-assisted method to introduce carbon-hydrogen (CH) units into WS monolayers. We found CH-groups to be the most stable dopant to introduce carbon into WS, which led to a reduction of the optical bandgap from 1.98 to 1.83 eV, as revealed by photoluminescence spectroscopy. Aberration corrected high-resolution scanning transmission electron microscopy (AC-HRSTEM) observations in conjunction with first-principle calculations confirm that CH-groups incorporate into S vacancies within WS. According to our electronic transport measurements, undoped WS exhibits a unipolar n-type conduction. Nevertheless, the CH-WS monolayers show the emergence of a p-branch and gradually become entirely p-type, as the carbon doping level increases. Therefore, CH-groups embedded into the WS lattice tailor its electronic and optical characteristics. This route could be used to dope other 2D-TMDs for more efficient electronic devices.
化学掺杂是改变二维过渡金属二硫属化物(2D-TMDs)电子、化学和光学性质的有效途径。我们采用等离子体辅助方法将碳氢(CH)单元引入WS单层。我们发现CH基团是将碳引入WS中最稳定的掺杂剂,光致发光光谱显示,这导致光学带隙从1.98 eV降低到1.83 eV。结合第一性原理计算的像差校正高分辨率扫描透射电子显微镜(AC-HRSTEM)观察证实,CH基团掺入WS中的S空位。根据我们的电子输运测量,未掺杂的WS表现出单极n型传导。然而,随着碳掺杂水平的增加,CH-WS单层出现了p分支,并逐渐完全变为p型。因此,嵌入WS晶格中的CH基团调整了其电子和光学特性。此途径可用于掺杂其他二维过渡金属二硫属化物,以制造更高效的电子器件。